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WO2025141340A1 - Technologie à émission nulle pour produire de l'énergie dans des centrales thermiques et de l'éther diméthylique à partir de dioxyde de carbone capturé - Google Patents

Technologie à émission nulle pour produire de l'énergie dans des centrales thermiques et de l'éther diméthylique à partir de dioxyde de carbone capturé Download PDF

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WO2025141340A1
WO2025141340A1 PCT/IB2024/060361 IB2024060361W WO2025141340A1 WO 2025141340 A1 WO2025141340 A1 WO 2025141340A1 IB 2024060361 W IB2024060361 W IB 2024060361W WO 2025141340 A1 WO2025141340 A1 WO 2025141340A1
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dme
gas
reaction
reactor
conversion
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Chandrashekar Jagannath Kargudri
Bhargavi Yedaguri Reddy
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    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
    • C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
    • C01B3/38—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts
    • C01B3/382—Multi-step processes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/02—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by adsorption, e.g. preparative gas chromatography
    • B01D53/04—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by adsorption, e.g. preparative gas chromatography with stationary adsorbents
    • B01D53/047—Pressure swing adsorption
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/14—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by absorption
    • B01D53/1456—Removing acid components
    • B01D53/1475—Removing carbon dioxide
    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C41/00—Preparation of ethers; Preparation of compounds having groups, groups or groups
    • C07C41/01—Preparation of ethers
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10K—PURIFYING OR MODIFYING THE CHEMICAL COMPOSITION OF COMBUSTIBLE GASES CONTAINING CARBON MONOXIDE
    • C10K3/00—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide
    • C10K3/02—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide by catalytic treatment
    • C10K3/026—Increasing the carbon monoxide content, e.g. reverse water-gas shift [RWGS]
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
    • F02C—GAS-TURBINE PLANTS; AIR INTAKES FOR JET-PROPULSION PLANTS; CONTROLLING FUEL SUPPLY IN AIR-BREATHING JET-PROPULSION PLANTS
    • F02C6/00—Plural gas-turbine plants; Combinations of gas-turbine plants with other apparatus; Adaptations of gas-turbine plants for special use
    • F02C6/18—Plural gas-turbine plants; Combinations of gas-turbine plants with other apparatus; Adaptations of gas-turbine plants for special use using the waste heat of gas-turbine plants outside the plants themselves, e.g. gas-turbine power heat plants
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/50—Carbon oxides
    • B01D2257/504—Carbon dioxide
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
    • C01B2203/0227—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step
    • C01B2203/0233—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step the reforming step being a steam reforming step
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
    • C01B2203/0227—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step
    • C01B2203/0244—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step the reforming step being an autothermal reforming step, e.g. secondary reforming processes
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/06—Integration with other chemical processes
    • C01B2203/062—Hydrocarbon production, e.g. Fischer-Tropsch process
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/10—Catalysts for performing the hydrogen forming reactions
    • C01B2203/1041—Composition of the catalyst
    • C01B2203/1047—Group VIII metal catalysts
    • C01B2203/1052—Nickel or cobalt catalysts
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/10—Catalysts for performing the hydrogen forming reactions
    • C01B2203/1041—Composition of the catalyst
    • C01B2203/1047—Group VIII metal catalysts
    • C01B2203/1064—Platinum group metal catalysts
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
    • C01B2203/1205—Composition of the feed
    • C01B2203/1211—Organic compounds or organic mixtures used in the process for making hydrogen or synthesis gas
    • C01B2203/1235—Hydrocarbons
    • C01B2203/1241—Natural gas or methane
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
    • C01B2203/1258—Pre-treatment of the feed
    • C01B2203/1264—Catalytic pre-treatment of the feed
    • C01B2203/127—Catalytic desulfurisation
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/14—Details of the flowsheet
    • C01B2203/142—At least two reforming, decomposition or partial oxidation steps in series
    • C01B2203/143—Three or more reforming, decomposition or partial oxidation steps in series

Definitions

  • US9803142B1 discloses catalysts and processes for converting DME and/or methanol to liquid fuels with high selectivity and yield. Main difference with the instant invention is that this Patent focuses on converting DME/methanol to liquid fuels rather than the initial production from CO 2 in a power generation context.
  • US7378561B2 teaches a method for producing methanol and dimethyl ether using air as the sole source of materials. Here the applicant describes a method for producing methanol and DME from atmospheric air using hydrogen produced by electrolysis. This Patent uses air as the source and focuses on electrolysis, differing from the integrated power generation and CO 2 capture approach.
  • US7846978B2 discloses a method of producing methanol from a methane source.
  • the first step involves using advanced power generation technologies like CCUS (Carbon Capture, Utilization, and Storage) systems that ensure minimal to zero emissions when burning natural gas which are highly efficient and can achieve lower emissions up to 94% than normal Greenhouse Gas (GHG) Emissions that refer to gases in the Earth's atmosphere that trap heat, contributing to the greenhouse effect and global warming.
  • CCUS Carbon Capture, Utilization, and Storage
  • This exothermic reaction generates carbon dioxide (CO2), water (H2O), and a substantial amount of heat.
  • the balanced chemical equation for this combustion reaction is: CH 4 +2O 2 ⁇ CO 2 +2H 2 O
  • the heat is used to generate electricity in a gas turbine, while the waste heat is further utilized in a Heat Recovery Steam Generator (HRSG) to produce steam for a steam turbine, maximizing energy extraction.
  • HRSG Heat Recovery Steam Generator
  • the CO2 produced during combustion is captured using advanced CO2 capture technologies, reducing greenhouse gas emissions. The integration of these processes results in an efficient and environmentally friendly power generation system. Thermal power plants producing bulk power emit CO2, and capturing these emissions requires a two-stage carbon capture process.
  • the first stage involves Pressure Swing Adsorption (PSA), widely used for separating gases in industrial processes, followed by the purification of the CO2 using a Monoethanolamine (MEA) solution.
  • PSA Pressure Swing Adsorption
  • MEA Monoethanolamine
  • the captured CO2 is then used in the following processes to achieve Net Zero Emissions (NZE).
  • Post-Capture Process Steps 1. Hydrogen Generation via Steam Methane Reforming (SMR) ( Figure 3) The process begins with hydrogen generation through Steam Methane Reforming (SMR) of natural gas in the presence of a catalyst: CH 4 + H 2 O ⁇ CO + 3H 2 2.
  • Reverse Water Gas Shift (RWGS) Reaction Figure 2) In the RWGS reaction furnace, waste CO2 and renewable H2 are introduced through their respective inlets.
  • the CO2 reacts with H2 at high temperatures (above 900°C) in the presence of an oxy-hydrogen flame, producing CO and H2O as per the following equation: CO 2 + H 2 ⁇ CO + H 2 O
  • the reaction is facilitated by the specific design of the furnace, that incorporates thermal insulation to retain heat and a heat exchanger to enhance energy efficiency by using the excess heat of this reaction for steam methane reforming.
  • the non-catalytic, thermally isolated environment allows for rapid CO2 conversion, with up to 75% efficiency achieved in less than 0.03 seconds.
  • the resulting syngas, composed of CO and H2O is then collected through the outlet for further processing in steam Methane reforming.
  • SMR Steam Methane Reforming
  • Figure 3 Methane and steam, along with about 25% residual CO2 and the shifted gases (CO and H2), are passed through a Steam Methane Reformer (SMR) at an inlet temperature of 525°C and 25 ATA pressure over metal catalysts including base metals (Ni, Co, Fe) and noble metals (Pt, Ir, Rh, Ru).
  • SMR Steam Methane Reformer
  • ATR Auto-Thermal Reforming Reactor
  • the SMR reaction conditions include desulfurization with ActiSorb G1M ZnO catalyst, followed by the steam reforming reaction: CH4 + H2O ⁇ CO + 3H2 A portion of the hydrogen is recycled (approximately 4 mol%) and separated using Pressure Swing Adsorption (PSA), a technology that separates gas species under pressure according to molecular characteristics. 4. Auto-Thermal Reforming Reactor (ATR) The gases from the SMR are further processed in an Auto-Thermal Reforming Reactor (ATR), a chemical reactor used to produce synthesis gas (syngas), which is a mixture of hydrogen (H2) and carbon monoxide (CO).
  • ATR Auto-Thermal Reforming Reactor
  • the reaction conditions are as follows: ⁇ Inlet Temperature: 700°C ⁇ Outlet Temperature: 975°C ⁇ Air Inlet Temperature: 230°C ⁇ Air Flow: 14 mol/hr ⁇
  • the outlet gas composition in mol% is as follows: ⁇ CH4: 0.4, CO: 17.879, CO2: 10.436, H2: 71.108, N2: 0.177 ⁇
  • the total dry gas flow is 134.829 kmol/hr with a steam flow of 91.336 kmol/hr.
  • the catalyst volumes are 0.5 m3, consisting of nickel-based catalyst, Refor-Max 420 (0.115 m3) at the top and another nickel-based catalyst, Refor-Max 330 (0.385 m3) at the bottom.
  • the DME synthesis reaction represents a novel and innovative approach in green energy and sustainable chemistry, converting CO2 directly into a clean fuel, DME.
  • the reaction is best performed at 25-40 ATA and 250°C-300°C in the presence of a suitable catalyst.
  • the output is 92 kg DME (579,600 Kcal), resulting in an Energy Efficiency Factor (EEF) of 93.04%.
  • DME Reactor-1 Regulated syngas temperature to 250°C and regulated pressure to 30 bar 6.
  • DME Reactor-2 Complete conversion of the remaining syngas to DME under the above conditions 7.
  • Distillation Column No.1 Separation of DME, methanol, and water 8.
  • DME Synthesis: 2CH 3 OH CH 3 OCH 3 + H2O 5.
  • the instant invention discloses a method for producing power in a thermal plant and synthesizing Dimethyl Ether (DME) from captured carbon dioxide (CO2), comprising the steps of: a) combusting natural gas (NG) (101) or liquefied natural gas (LNG) in a gas combustor (103) to generate electricity and produce flue gases containing CO2, wherein the natural gas comprises primarily methane (CH4); b) capturing the CO2 from the flue gases using a two-stage carbon capture process , consisting of a Pressure Swing Adsorption (PSA) system (106), followed by purification using a Monoethanolamine (MEA) solution to achieve a purity of captured CO2 of at least 95%; c) converting the captured CO2 into carbon monoxide (CO) through a Reverse Water Gas Shift (RWGS) reaction, in a RWGS Reaction Furnace (306), wherein, the reaction is performed in a non-catalytic furnace with an oxy-hydrogen flame at a temperature above
  • ATR Auto-Thermal Reforming
  • the RWGS reaction achieves a CO2 conversion efficiency between 48% and 60% with a hydrogen consumption minimized to 1 mol H2 per mol CO2, facilitated by integrated heat recovery in an insulated industrial reactor.
  • the PSA system optimizes the H2/CO ratio to approximately 2:1 for DME synthesis, ensuring minimal excess hydrogen.
  • the second SMR reactor operates at an inlet temperature 525°C, an outlet temperature of 900°C, and a pressure of 25 ATA over a metal catalyst selected from the group consisting of Ni, Co, Fe, Pt, Ir, Rh, and Ru.
  • the gas composition is : CH4: 15.399%, CO: 8.105%, CO2: 11.242%, H2: 65.040%, and N2: 0.213%.
  • the ATR reactor produces a syngas mixture with the following outlet composition: CH4: 0.4%, CO: 17.879%, CO2: 10.436%, H2: 71.108%, N2: 0.177%, with a total dry gas flow of 134.829 kmol/hr and a steam flow of 91.336 kmol/hr.
  • Said DME synthesis reactors achieve a conversion efficiency of up to 85% in a single pass, with a final yield of 92 kg DME per 48 kg LNG input, and an energy efficiency factor (EEF) of 93.04%.
  • the CO2 captured from the flue gases is processed in the RWGS reaction with a heat input sufficient to maintain the reaction temperature above 900°C, supplied by the combustion of 2 moles of hydrogen per mole of CO2.
  • the first distillation column provided therein separates DME from methanol and water at a pressure of 30 bar, and the second distillation column further purifies methanol and water.
  • the instant process achieves an overall energy efficiency of 90% or higher, and the CO2 reduction footprint is -63 grams CO2 e/MJ of DME produced, achieving a 94% abatement of greenhouse gases.
  • FIG. 2 shows the Reverse Water Gas Shift (RWGS) reaction furnace to convert waste CO 2 and renewable H 2 to CO and H 2 O, wherein 201- O2/CO2 Inlet; 202- H2 Inlet; 203- Reaction Furnace; 204- Oxy-Hydrogen Flame; 205- CO and H2O Outlet; and 206- Insulation.
  • RWGS Reverse Water Gas Shift

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Combustion & Propulsion (AREA)
  • General Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Analytical Chemistry (AREA)
  • Mechanical Engineering (AREA)
  • General Engineering & Computer Science (AREA)
  • Health & Medical Sciences (AREA)
  • General Health & Medical Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Hydrogen, Water And Hydrids (AREA)

Abstract

L'invention concerne une technologie à émission nulle pour produire de l'énergie dans une centrale thermique à l'aide de gaz naturel (NG) ou de gaz naturel liquéfié (GNL), suivi par la capture de dioxyde de carbone (CO2) et la conversion de celui-ci en diméthyléther (DME) vert. Le procédé intègre une centrale électrique à cycle combiné à base de gaz avec une capture de CO2 par adsorption modulée en pression (PSA) (106) et une purification de monoéthanolamine (MEA). Le CO2 capturé subit une réaction de conversion de gaz à l'eau inverse (RWGS) (306) à des températures supérieures à 900 °C pour former du CO, qui, conjointement avec du gaz de synthèse provenant du reformage de méthane à la vapeur (308a, 308) à 525-900 °C et à une pression de 25 ATA, est converti en DME à l'aide d'un catalyseur Cu/ZnO/Al2O3 à 250-300 °C et 25-40 ATA. Le procédé permet d'obtenir un facteur d'efficacité énergétique de 93,04 %, produisant 92 kg de DME pour 48 kg de GNL, avec une réduction de 94 % de gaz à effet de serre, contribuant à des émissions nettes nulles (NZE) tout en générant une puissance thermique en vrac.
PCT/IB2024/060361 2023-12-28 2024-10-22 Technologie à émission nulle pour produire de l'énergie dans des centrales thermiques et de l'éther diméthylique à partir de dioxyde de carbone capturé Pending WO2025141340A1 (fr)

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IN202341065407 2023-12-28

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Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US8133926B2 (en) * 2007-06-21 2012-03-13 University Of Southern California Conversion of carbon dioxide to dimethyl ether using bi-reforming of methane or natural gas

Patent Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US8133926B2 (en) * 2007-06-21 2012-03-13 University Of Southern California Conversion of carbon dioxide to dimethyl ether using bi-reforming of methane or natural gas

Non-Patent Citations (2)

* Cited by examiner, † Cited by third party
Title
CATIZZONE ENRICO, BONURA GIUSEPPE, MIGLIORI MASSIMO, FRUSTERI FRANCESCO, GIORDANO GIROLAMO: "CO2 Recycling to Dimethyl Ether: State-of-the-Art and Perspectives", MOLECULES, MDPI AG, CH, vol. 23, no. 1, CH , pages 31, XP093333857, ISSN: 1420-3049, DOI: 10.3390/molecules23010031 *
POTO SERENA, GALLUCCI FAUSTO, FERNANDA NEIRA D'ANGELO M.: "Direct conversion of CO2 to dimethyl ether in a fixed bed membrane reactor: Influence of membrane properties and process conditions", FUEL, IPC SIENCE AND TECHNOLOGY PRESS , GUILDFORD, GB, vol. 302, 1 October 2021 (2021-10-01), GB , pages 121080, XP093333852, ISSN: 0016-2361, DOI: 10.1016/j.fuel.2021.121080 *

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